This study aims to evaluate the use of sugarcane industry byproducts (bagasse and molasses), as well as glycerol from the liquor of the organosolv pretreatment of bagasse, to bioproduce 1,3-propanediol (1,3-PDO). For this purpose, Lentilactobacillus diolivorans was used, which can produce 1,3-PDO from a mixture of glycerol and sugars. First, experiments were conducted using the MRS medium to investigate the effect of various carbohydrate sources and their mixtures on the growth profile and 1,3-PDO production by L. diolivorans. Subsequently, the carbohydrates in the MRS medium were replaced with sugarcane byproducts. The results showed that the type of carbohydrate plays a crucial role in growth kinetics and 1,3-PDO production. Xylose and glucose showed the best results; however, sucrose was not enough to support biomass formation. The presence of xylose increased sucrose assimilation, resulting in a 4.5-fold increase in the concentration of 1,3-PDO from 1.3 to 6.18 g/L. An auspicious outcome was observed when the liquor of the acid pretreatment of sugarcane bagasse, molasses, and organosolv liquor were used as substrates, resulting in a production of 5.47 g/L 1,3-PDO with an efficiency of 82.77%. Therefore, producing a high-value chemical such as 1,3-PDO from the sugarcane byproducts seems to be a very promising strategy.